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Analysis of Dyes in Cosmetics: Challenges and Recent Developments

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Analysis of Dyes in Cosmetics: Challenges and Recent Developments cosmetics Review Analysis of Dyes in Cosmetics: Challenges and Recent Developments Eugenia Guerra, Maria Llompart ID and Carmen Garcia-Jares * Laboratory of Research and Development of Analytical Solutions (LIDSA), Department of Analytical Chemistry, Nutrition and Food Science, Faculty of Chemistry, Universidade de Santiago de Compostela, E-15782 Santiago de Compostela, Spain; [email protected] (E.G.); [email protected] (M.L.) * Correspondence: [email protected]; Tel.: +34-8818-14394 Received: 4 July 2018; Accepted: 20 July 2018; Published: 23 July 2018 Abstract: Colour plays a decisive role in the marketing of a cosmetic product. Among thousands of substances used to colour, synthetic dyes are the most widespread in the industry. Their potential secondary effects on human health and different regulatory requirements for their use between the main world markets make analytical control necessary to guarantee the safety of a cosmetic product. However, methodologies for the determination of dyes in cosmetics are scarce with respect to those reported for other cosmetic ingredients such as preservatives or ultraviolet UV filters. In addition, most of the existing methods just consider a part of the total of dyes regulated. On the other hand, many methods have been developed for matrices different than cosmetics such as foodstuff, beverages or wastewater. The current paper reviews the recent developments in analytical methodologies for the control of synthetic dyes in cosmetics proposed in the international scientific literature in the last 10 years (2008–2018). A trend towards the use of miniaturized extraction techniques is evidenced. Due to the hydrophilic nature of dyes, liquid chromatography is the most usual choice in combination with absorbance detectors and, more recently, with mass spectrometry. Keywords: cosmetics; dyes; cosmetics analysis; sample preparation; matrix solid-phase dispersion; miniaturized extraction techniques; liquid chromatography; mass spectrometry; cosmetics safety 1. Introduction Colour is a key property of a product to determine the attractiveness for consumers and, therefore, its successful marketing. Colouring agents can be added to cosmetics in order to colour the product itself or to colour a part of the body (skin, hair, nails or eyelashes). In this latter case, the so-called colour cosmetic is a sector with a strong growth in the industry of cosmetics, given the increasing concern with body image motivated by the popularity of social media [1]. According to their use, cosmetics can be classified as leave-on, those that are in prolonged contact with the skin such as lipstick, cream or body lotion, and rinse-off, those that are removed after application such as shampoo, gel or soap. Colorants can be classified according to their structure, source, colour, solubility and application method [2]. Two main categories are established according to solubility: dyes and pigments. Dyes are synthetic organic compounds that are hydro or oil-soluble and they can be found in cosmetics such as skin care products or toiletries whereas pigments are insoluble, they remain in particulate form, and they are mainly employed in toothpastes or decorative make-up [3]. Among the thousands of substances employed as colouring agents, synthetic dyes are preferred over natural (obtained from plants, animals and minerals) given their lower production costs and long-lasting properties such as brightness or greater stability towards light, heat or pH extreme that may occur during the manufacturing process. They can also be classified according to chemical Cosmetics 2018, 5, 47; doi:10.3390/cosmetics5030047 www.mdpi.com/journal/cosmetics Cosmetics 2018, 5, 47 2 of 15 structure in five main groups: azoic, triarylmethane, xanthenes, indigoid and quinoline. Table1 shows examples of dyes belonging to each structural family and the corresponding range of Colour Index (CI) number. CI number is a code composed by five numbers used globally to identify these substances. The first two digits indicate the structural category of the dye. Sometimes, they are associated also to an E code, which means that they can be used as food additives. CosmeticsCosmetics 20182018 2018,,, ,55 5,,, ,xxx x FORFORFOR FOR PEERPEERPEER PEER REVIEWREVIEWREVIEW REVIEW 222 ofof of 1717 17 Table 1. Classification of dyes according to their chemical structure. TableTable 1. 1. Classification Classification of of dyes dyes according according to to their their chemical chemical structure. structure. CategoryCategoryCategory CI RangeCICI Range Range Example Example AzoAzoAzo 11XXX–35XXX11XXX–35XXX11XXX–35XXX CICI 19140 19140 Tartrazine Tartrazine TriarylmethaneTriarylmethaneTriarylmethane 42XXX–44XXX 42XXX–44XXX42XXX–44XXX CICI 42090 42090 Brilliant Brilliant Blue Blue XantheneXantheneXanthene 45XXX45XXX45XXX CICI 45410 45410 Acid Acid Red Red 92 92 QuinolineQuinolineQuinoline 47XXX47XXX47XXX CICI 47005 47005 Quinoline Quinoline Yellow Yellow IndigoidIndigoidIndigoidIndigoid 73XXX73XXX73XXX73XXX CICI 73015 73015 Indigotine Indigotine AmongAmong the the thousands thousands of of substances substances employedemployed employed asas as colouringcolouring colouring agents,agents, agents, syntheticsynthetic synthetic dyesdyes dyes areare are preferredpreferred preferred Azo dyes, synthesisedoverover natural natural from (obtained (obtained an aromatic from from plants, plants, amine, animals animals are by and and far minerals) minerals) the most given given used their their inlower lower any production production consumer costs costs product and and due to their lower price.long-lastinglong-lastinglong-lasting Their characteristic propertiesproperties properties suchsuch such asas aschromophoric brbr brightnessightnessightness oror or greatergreater greater azo stabilitystability stability group, towardstowards towards under light,light, light, determined heatheat heat oror or pHpH pH extremeextreme extreme conditions thatthat that may occur during the manufacturing process. They can also be classified according to chemical that can take place in intestinalmaymay occuroccur during bacteria,during thethe manufacturing livermanufacturing cells, and process.process. skin TheyThey surface cancan alsoalso micro bebe classifiedclassified flora [4 according],according may be toto reduced chemicalchemical to aromatic amines suspected to cause mutagenic, genotoxic and carcinogenic effects [5]. Although most of epidemiological studies are oriented towards azo dyes, there are also evidences of health risks of other families of colorants. The main route of human exposure to dyes in cosmetics is dermal contact, with special attention to areas close to mucous membranes such as eyes or lips where decorative make-up is daily applied. It has been proven that triarylmethanes are able to enter the blood stream Cosmetics 2018, 5, 47 3 of 15 after systemic absorption [6]. Another study pointed out genotoxic effects caused by the absorption though the skin of Quinoline Yellow [7]. Xanthenes dyes such as Acid Red 92, Erythrosine, or Rose Bengal, which are very popular in cosmetics due to the red shade formed, have been identified as responsible of the formation of rough skin by reacting with proteins on the skin [8]. For other colorants such as Rhodamine B, harmful effects evidenced [9] have led European Union EU authorities to ban the use of these substances in cosmetics. Among substances intended to colour hair, permanent or oxidative hair dyes are widely used, although they are known as strong allergens [10,11] and thus, the analytical control of these substances is a major concern [12]. However, they have not been considered in this review since they present a chemical nature completely different to synthetic dyes and hence other analytical approaches are needed for their determination in hair dyeing formulations [13]. Only synthetic dyes employed as temporary hair dyes have been included in the methodological review. On the other hand, it is worth mentioning that the colouring agents employed in tattoos and permanent make-up (PMU), this last consisting on semi (permanent) tattoos used to resemble make-up. The main components are pigments, though dyes are also employed in small amounts, particularly in the form of lake due to their stability. Over 80% of the colorants used are organic and more than 60% of them are azo-pigments, some of which can release aromatic amines as by-products or impurities from synthesis. Raw colour materials employed for tattoos and PMU are not specifically produced for this application, so their purity is generally low. Aromatic amines, polycyclic aromatic hydrocarbons (PAH) or heavy metals can be present and thus a comprehensive analytical control of ingredients as well as unwanted substances is highly needed. However, the lack of a European regulatory framework and harmonized analytical methodologies developed specifically for tattoos and PMU makes the control of these substances difficult and represents a concern that must be dealt with separately [14]. This paper reviews the analytical methodology and developments for the control of synthetic dyes in cosmetics reported in international scientific journals in the last 10 years (2008–2018). Analytical improvements made on both sample preparation and determination are discussed. Recent contributions in this field tended to the development of methods based on micro-extraction techniques and liquid chromatography coupled to mass spectrometry. 2. Regulatory Overview Dyes are subject to a wide
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